caa a22 4500 378927221 CHVBK 20180305123620.0 cr unu---uuuuu 161128e20041101xx s 000 0 eng 10.1524/ract.92.9.639.54976 doi (NATIONALLICENCE)gruyter-10.1524/ract.92.9.639.54976 Trivalent actinide coprecipitation with powellite (CaMoO4): Secondary solid solution formation during HLW borosilicate-glass dissolution [Elektronische Daten] [Dirk Bosbach, Thomas Rabung, Felix Brandt, Thomas Fanghänel] Powellite (CaMoO4) is one of the various crystalline secondary alteration phases which form during the corrosion of high level waste (HLW) glasses. Due to their structural variability, powellite can accommodate considerable chemical substitutions including trivalent actinides. Batch adsorption and coprecipitation experiments in mixed flow reactors have been used to study quantitatively the uptake of Cm(III) and Eu(III) (as a nonradioactive chemical homologue for trivalent actinides) from aqueous solution under repository relevant conditions. A metal ion concentration-independent Kd of 1200ml/g has been determined for adsorption above pH 4 up to 3μmol/L Eu(III). The partition coefficient for coprecipitation varies between 10 and 800 depending on the precipitation rate. Time-resolved laser fluorescence spectroscopy has been used to study the aqueous complexation of Cm(III)/Eu(III) and MoO42- as well as their incorporation into the powellite crystal lattice during coprecipitation. A red shift of the Cm(III) fluorescence emission of the transition indicates the formation of aqueous CmMoO4+ (598nm) and Cm(MoO4)22- (601nm) complexes. The incorporation of Cm(III) is indicated by a significant red shift. The corresponding lifetime of 165μs indicates quench effects. A similar behaviour has been observed for Eu(III). The life time of the 5D0-7F2 transition is 350μs for an incorporated Eu(III) species, suggesting also intrinsic quench effects, due to the local crystal field or impurities. © 2004 Oldenbourg Wissenschaftsverlag GmbH Laboratory techniques, experiments nationallicence Analytical chemistry nationallicence Inorganic chemistry nationallicence Bosbach Dirk aut Rabung Thomas aut Brandt Felix aut Fanghänel Thomas aut Radiochimica Acta/International journal for chemical aspects of nuclear science and technology Oldenbourg Wissenschaftsverlag GmbH 92/9-11/2004(2004-11-01), 639-643 0033-8230 92:9-11/2004<639 2004 92 ract https://doi.org/10.1524/ract.92.9.639.54976 text/html Onlinezugriff via DOI 1 research article jats NATIONALLICENCE 856 40 https://doi.org/10.1524/ract.92.9.639.54976 text/html Onlinezugriff via DOI NATIONALLICENCE 700 1- Bosbach Dirk aut NATIONALLICENCE 700 1- Rabung Thomas aut NATIONALLICENCE 700 1- Brandt Felix aut NATIONALLICENCE 700 1- Fanghänel Thomas aut NATIONALLICENCE 773 0- Radiochimica Acta/International journal for chemical aspects of nuclear science and technology Oldenbourg Wissenschaftsverlag GmbH 92/9-11/2004(2004-11-01), 639-643 0033-8230 92:9-11/2004<639 2004 92 ract CC0 http://creativecommons.org/publicdomain/zero/1.0 nationallicence BK010053 XK010053 XK010000 NATIONALLICENCE NATIONALLICENCE NL-gruyter